High-Dimensional Quantum Dynamics Study on Excitation-Specific Surface Scattering Including Lattice Effects of a Five-Atom Surface Cell.
High-Dimensional Quantum Dynamics Study on Excitation-Specific Surface Scattering Including Lattice Effects of a Five-Atom Surface Cell.
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DOI：
10.1021/acs.jctc.1c00241
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发表时间：
2021-03
影响因子：
5.5
通讯作者：
Qingyong Meng;Markus Schröder;H. Meyer
中科院分区：
文献类型：
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作者：
Qingyong Meng;Markus Schröder;H. Meyer
采用多层多组态含时Hartree（ML-MCTDH）方法，对一氧化碳分子在铜（100）表面上的模式特异性表面散射进行了高维（21 D）量子动力学计算.我们采用了一个表面模型，其中五个表面原子附近的影响网站被视为完全灵活的量子粒子，而所有其他更遥远的原子保持在固定的位置。为了有效地执行21维ML-MCTDH波包传播，势能面被转移到一个典型的多矢分解形式与基于蒙特卡洛的方法的帮助。计算了CO在Cu（100）表面上的激发态特异性吸附几率，并与刚性表面的吸附几率进行了比较，证明了柔性表面原子引起的晶格效应。研究了系统初始态的粘附几率的依赖关系，发现碰撞点表面原子初始振动激发时，粘附几率降低。
In this work, high-dimensional (21D) quantum dynamics calculations on the mode-specific surface scattering of a carbon monoxide molecule on a copper(100) surface with lattice effects of a five-atom surface cell are performed through the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method. We employ a surface model in which five surface atoms near the impact site are treated as fully flexible quantum particles, while all other more distant atoms are kept at fixed locations. To efficiently perform the 21D ML-MCTDH wave packet propagation, the potential energy surface is transferred to a canonical polyadic decomposition form with the aid of a Monte Carlo-based method. Excitation-specific sticking probabilities of CO on Cu(100) are computed, and lattice effects caused by the flexible surface atoms are demonstrated by comparison with sticking probabilities computed for a rigid surface. The dependence of the sticking probability of the initial state of the system is studied, and it is found that the sticking probability is reduced when the surface atom on the impact site is initially vibrationally excited.